The molecular-scale self-assembly of a 3D aluminosiloxane (Al-O-Si) hybrid gel network was successfully performed via the cocondensation of hydrolyzed alumina (AlOOH) and (3-aminopropyl)trimethoxysilane (APS). It was transformed into a microspherical aerogel framework of Al-O-Si containing mesochannels with tunable hierarchically bimodal meso/macroporosities by a subcritical drying technique. Good homogeneity of AlOOH and APS brought during the synthesis guaranteed a uniform distribution of two metal oxides in a single body. A systematic characterization of the aerogel support was carried out using FTIR, SEM, TEM, nitrogen adsorption/desorption analysis, WAXS, SAXS, and ξ-potential measurement in order to explore the material for drug uptake and release. The drug loading and release capacity and chemical stability of an aluminosiloxane aerogel were studied using two nonsteroidal antiinflammatory drugs, ibuprofen and aspirin. A comprehensive evaluation of the aluminosiloxane aerogel with ordered mesoporous MCM-41 was also performed. Aerogel supports showed a high drug loading capacity and a pH-responsive controlled-release property compared to MCM-41. Meanwhile, kinetic modeling studies indicate that the drug releases with a zero-order profile following the Korsmeyer-Peppas model. The biocompatibility of aluminosiloxane aerogels was established via ex vivo and in vivo studies. We also outline the use of aluminosiloxane aerogel as a support for a possible 3D matrix for an osteoconductive structure for bone tissue engineering.
The supramolecular assembly of stimuli-responsive gels is renowned in organic, polymeric and biological systems, but it is seldom reported in inorganic gel systems. Here we report the inorganic system aluminosiloxane (ALS) aquagel by sol-gel synthesis that shows a unique mechano-responsive property with an impressive recovery rate. An assembly of 2D nanoribbon/tape like structural architectures was distinctively identified as the primary building block of the aquagel structure. This fascinating 2D architecture selfassembled into a well-defined 3D porous aquagel cage via weak supramolecular interactions. This is identified to be an excellently mechanically stable, injectable and non-cytotoxic medium for drug delivery applications. The ALS aquagel can also overcome the untoward effects caused by photoinitiators, chemical cross-linking agents and organic solvents in organo/polymeric gels when it is used for biomedical applications. Herein, we successfully utilized the ALS inorganic aquagel for the encapsulation and sustained release of fluconazole (FLZ), an antifungal drug, for the first time. The FLZ loaded aquagel showed good antifungal susceptibility against various fungi species, such as Candida albicans, Candida tropicalis and Trichophyton rubrum. The FLZ-ALS aquagel showed an eight-fold enhancement in antifungal susceptibility against the most threatening Candida fungi species when compared to the marketed formulation.
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